Multi‐atom catalysts exhibit complex intermetallic and metal‐ligand interactions. Traditional local descriptors fail to capture the global electronic characteristics, limiting the rational design of efficient electrocatalysts. Herein, an aromatic resonance (
A
R
) index is introduced as a global descriptor to assess the catalytic performance of multi‐atom catalysts, with the electrochemical carbon monoxide reduction reaction as a representative case study. Unlike local descriptors,
A
R
index quantitatively describes the dynamic “electronic buffer” formed by the π‐electron delocalization network within the ligand framework, showing a clear linear relationship with the Gibbs free energy change of a potential‐determining step (PDS). Mechanistic insights reveal that decreased
A
R
index disrupts global delocalization, enhances metal‐ligand coupling, and promotes C─O bond activation. Guided by
A
R
, Cu
2
TiN
6
@graphene is identified as the optimal catalyst, with a PDS of 0.17 eV and a kinetic barrier of 0.64 eV. This work provides an effective global perspective for understanding structure‐performance relationships in complex multi‐atom electrocatalysts.
Well-defined active sites and tunable electronic features of single-atom catalysts (SACs) enable great versatility in modulating their electrocatalytic activity. However, an understanding of how the electronic structure governs the catalytic efficiency and product selectivity for CO2 and O2 reduction reactions (CO2RR a...
Y. K. Sahana, Vasanthapandiyan Mari, Naiwrit Karmodak· Chemical Communications· 0 citations
The oxygen reduction reaction (ORR) is a central process in energy conversion and storage systems, such as fuel cells and metal–air batteries. To meet the urgent demand for efficient ORR catalysts, promising single-atom catalysts (SACs) with heteroatoms incorporated into a carbon matrix are a current research focus....
Han Zhao, Ze-Yi Zhang, Jing-Kai Lin et al.· ACS Catalysis· 0 citations
Electrochemical nitrogen reduction reaction (eNRR) offers a sustainable pathway for ammonia synthesis under ambient conditions; however, its practical implementation remains hindered by the inertness of the NN bond, limited N2 activation, and the competing hydrogen evolution reaction (HER). Single-atom catalysts (SACs...
The activation of peroxymonosulfate (PMS) for selective oxidant generation in advanced oxidation process is a sought objective when using single-atom catalysts (SACs) over conventional nanomaterials. However, challenges in controlling atomic-level morphology and understanding the intricate interplay between electronic...
Yi-Fei Wang, Xuedi Sun, Hao Wang et al.· Science Advances· 0 citations
The catalytic performance of single‐atom catalysts (SACs) is critically shaped by their local chemical environment, yet the role of structural features beyond the first coordination shell remains poorly understood. Here, we employ Ir single‐atom‐loaded ZnCo
2
O
4
spinel oxides with calcination‐tuned Co spin‐sta...
Cun-Yuan Gao, Shi-Yu Zhen, Yu-Tong Wang et al.· Advanced Energy Materials· 0 citations
Efficient multielectron electrocatalysis in layered covalent organic frameworks (COFs) is frequently limited by weak cross‐plane charge delivery to pore‐confined active sites. Herein, we report the construction of two metal‐bridged COFs (Py1‐COF‐Cu and Py2‐COF‐Cu) by incorporating nitrogen‐containing heterocycles to fa...
